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Abstract: The buried interface tens of nanometers beneath the solid-liquid junction is crucial for photocarrier extraction, influencing the overall efficiency of photoelectrochemical devices. Precise characterization of the interfacial properties is essential for device optimization but remains challenging. Here, we directly probe the in situ transformation of a CuxO interlayer at the NiO/n-Si interface by hard X-ray photoelectron spectroscopy. It is found that Cu(I) in the CuxO interlayer gradually transforms to Cu(II) with air exposure, forming an energetically more favorable interface and improving photoanode’s efficiency. Based on this finding, a reactive e-beam evaporation process is developed for the direct deposition of a CuO interlayer, achieving a half-cell solar-to-hydrogen efficiency of 4.56% for the optimized NiO/CuO/n-Si heterojunction photoanode. Our results highlight the importance of precision characterization of interfacial properties with advanced hard X-ray photoelectron spectroscopy in guiding the design of efficient solar water-splitting devices.
Keywords: photo anode, energy harvesting, nickel oxide, interface
Published in RUNG: 01.08.2024; Views: 620; Downloads: 8
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Abstract: I will present a study I conducted with Furkan Dikmen and Ömer Demirok on the semantic and pragmatic properties of the Turkish ‘discourse partıcle’ hani. On the one hand, the function of hani is merely pragmatic, on the other hand, it is subject to the truth-conditional effect of other constituents at LF. In this study, we introduce the first formal semantic and pragmatic treatment of clauses containing hani. Unlike previous accounts (see Erguvanlı-Taylan (Studies on Turkish and Turkic languages; proceedings of the ninth international conference on Turkish linguistics, 133–143, 2000), Akar et al. (Discourse meaning, 57–78, 2020), and Akar and Öztürk (Information-structural perspectives on discourse particles, 251–276, 2020), we claim that hani can have one of the following two major pragmatic functions: making salient a proposition in the Common Ground or challenging one in a past Common Ground, therefore requiring a Common Ground revision. Despite its variety of occurrences, we argue that hani has a uniform interpretation and provide a compositional analysis of the different construals that it is associated with. Furthermore, we show that a formally explicit and accurate characterization of hani-clauses requires operating on indexical parameters, in particular the context time. Therefore, if our proposal is on the right track, hani clauses may provide indirect empirical evidence in favour of the existence of “monstrous” phenomena, adding to the accumulating cross-linguistic evidence in this domain (see Schlenker in Linguistics and Philosophy 26(1):29–120, 2003 and much work since then). The definition of monsters is intended as in Kaplan (Themes from Kaplan, 481–563, 1989).
Keywords: Semantics, Turkish, Discourse Particle, Temporal Shift
Published in RUNG: 31.07.2024; Views: 571; Downloads: 0
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Keywords: oxidation mechanism, surface core level shift, density functional theory, surface reconstruction, magnesium oxidation
Published in RUNG: 25.07.2024; Views: 655; Downloads: 3
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Keywords: nanobodies, extracellular vesicles, immunoaffinity purification
Published in RUNG: 23.07.2024; Views: 619; Downloads: 5
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Abstract: Particle size is an important physical parameter in any nanomaterial designed for biomedical applications. It critically influences the biological fate of nanoparticles. It is generally believed that a range between 10 and 200 nm is most relevant to physical and biochemical targeting through both intravascular and site-specific deliveries.1 High porosity, purely organic nature, structural tunability and the ability to gradually release therapeutically-relevant cargo have rendered covalent organic frameworks (COFs) promising materials in biomedical research. While several COF-based drug delivery systems have been reported, particle aggregation and the associated particle size pose a significant barrier to real-life implementation of these systems.2 In the current talk, two strategies to address these issues will be presented as they have been applied to biosensing and delivery applications. Firstly, prolonged ultrasonication has proven an effective method of reducing the COF particle size while maintaining the material’s chemical properties.3 A fluorescent COF, that was post-synthetically modified to incorporate a hypoxia-targeting nitroimidazole moiety, was exposed to prolonged ultrasonication which effectively reduced the particle size from several µm to <170 nm.4 The ultrasonication treatment did not significantly hamper the material’s physical or chemical properties, such as crystallinity, and it even enhanced its fluorescence signal by overcoming aggregation-caused quenching (ACQ). The material and its constituent building blocks were shown to have minimal or no cytotoxicity. The COF’s internalization was monitored by fluorescence spectroscopy, and it preferentially accumulated in cells exposed to hypoxic environment, thus serving as a fluorescent biosensor for hypoxia. Another strategy of limiting the COF particle size is to grow the material on nano-sized substrates. Silver nanowires (AgNWs) have been shown as effective intracellular sensors5 and single-cell endoscopic tools.6 We have prepared AgNWs with diameters below 200 nm and have employed various synthetic methods to coat them with thiol-functionalized COFs. Favorable coordination bonds that form between Ag and the thiol functional group in the COF linkers drive the assembly process. Both bottom-up synthetic approaches, where the COF is grown on the surface of AgNWs, and top-down strategies, where pre-synthesized COF particles are attached onto AgNWs surface have been successful. The inorganic-organic hybrid materials were characterized by various techniques, including electron microscopy, Fourier-transform infrared spectroscopy, thermogravimetric analysis, and powder X-ray diffraction. All characterizations combined suggest that the diameter of the COF-coated AgNWs remains well in the nanometer-size regime. References: (1) Hickey, J. W.; Santos, J. L.; Williford, J.-M.; Mao, H.-Q. Control of Polymeric Nanoparticle Size to Improve Therapeutic Delivery. J. Control. Release 2015, 219, 536–547. (2) Esrafili, A.; Wagner, A.; Inamdar, S.; Acharya, A. P. Covalent Organic Frameworks for Biomedical Applications. Adv. Healthc. Mater. 2021, 10 (6), 2002090. (3) Skorjanc, T.; Heinrich, J.; Makuc, D.; Kulak, N.; Valant, M. Sustained Delivery of Cu(II)-Based DNA Intercalators by Nanometer-Sized Cyclodextrin-Based Porous Polymers. ACS Appl. Nano Mater. 2023, 6 (22), 21162–21168. (4) Skorjanc, T.; Shetty, D.; Kumar, S.; Makuc, D.; Mali, G.; Volavšek, J.; Bergant Marušič, M.; Valant, M. Nitroreductase-Sensitive Fluorescent Covalent Organic Framework for Tumor Hypoxia Imaging in Cells. Chem. Commun. 2023, 59 (38), 5753–5756. (5) Zhang, Q.; Inose, T.; Ricci, M.; Li, J.; Tian, Y.; Wen, H.; Toyouchi, S.; Fron, E.; Ngoc Dao, A. T.; Kasai, H.; Rocha, S.; Hirai, K.; Fortuni, B.; Uji-i, H. Gold-Photodeposited Silver Nanowire Endoscopy for Cytosolic and Nuclear PH Sensing. ACS Appl. Nano Mater. 2021, 4 (9), 9886–9894. (6) Ricci, M.; Fortuni, B.; Vitale, R.; Zhang, Q.; Fujita, Y.; Toyouchi, S.; Lu, G.; Rocha, S.; Inose, T.; Uji-I, H. Gold-Etched Silver Nanowire Endoscopy: Toward a Widely Accessible Platform for Surface-Enhanced Raman Scattering-Based Analysis in Living Cells. Anal. Chem. 2021, 93 (12), 5037–5045.
Keywords: covalent organic frameworks, imaging, delivery, nanoendoscopy, nanowire
Published in RUNG: 22.07.2024; Views: 608; Downloads: 2
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